Backbone NxH compounds at high pressures

Alexander F. Goncharov; Nicholas Holtgrewe; Guangrui Qian; Chaohao Hu; Artem R. Oganov; Maddury Somayazulu; Elissaios Stavrou; Chris J. Pickard; Adam Berlie; Fei Yen; Mahmood Mahmood; Sergey S. Lobanov; Zuzana Konôpková; Vitali B. Prakapenka

doi:10.1063/1.4922051

Backbone N_xH compounds at high pressures

Alexander F. Goncharov, Nicholas Holtgrewe, Guangrui Qian, Chaohao Hu, Artem R. Oganov, Maddury Somayazulu, Elissaios Stavrou, Chris J. Pickard, Adam Berlie, Fei Yen, Mahmood Mahmood, Sergey S. Lobanov, Zuzana Konôpková, Vitali B. Prakapenka

Research output: Contribution to journal › Article › peer-review

37 Scopus citations

Abstract

Optical and synchrotron x-ray diffraction diamond anvil cell experiments have been combined with first-principles theoretical structure predictions to investigate mixtures of N₂ and H₂ up to 55 GPa. Our experiments show the formation of structurally complex van der Waals compounds [see also D. K. Spaulding et al., Nat. Commun. 5, 5739 (2014)] above 10 GPa. However, we found that these N_xH (0.5 < x < 1.5) compounds transform abruptly to new oligomeric materials through barochemistry above 47 GPa and photochemistry at pressures as low as 10 GPa. These oligomeric compounds can be recovered to ambient pressure at T < 130 K, whereas at room temperature, they can be metastable on pressure release down to 3.5 GPa. Extensive theoretical calculations show that such oligomeric materials become thermodynamically more stable in comparison to mixtures of N₂, H₂, and NH₃ above approximately 40 GPa. Our results suggest new pathways for synthesis of environmentally benign high energy-density materials. These materials could also exist as alternative planetary ices.

Original language	English
Article number	214308
Journal	Journal of Chemical Physics
Volume	142
Issue number	21
DOIs	https://doi.org/10.1063/1.4922051
State	Published - 5 Jun 2015
Externally published	Yes

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@article{ce316441b4534ab5ac2aed08fc266b32,

title = "Backbone NxH compounds at high pressures",

abstract = "Optical and synchrotron x-ray diffraction diamond anvil cell experiments have been combined with first-principles theoretical structure predictions to investigate mixtures of N2 and H2 up to 55 GPa. Our experiments show the formation of structurally complex van der Waals compounds [see also D. K. Spaulding et al., Nat. Commun. 5, 5739 (2014)] above 10 GPa. However, we found that these NxH (0.5 < x < 1.5) compounds transform abruptly to new oligomeric materials through barochemistry above 47 GPa and photochemistry at pressures as low as 10 GPa. These oligomeric compounds can be recovered to ambient pressure at T < 130 K, whereas at room temperature, they can be metastable on pressure release down to 3.5 GPa. Extensive theoretical calculations show that such oligomeric materials become thermodynamically more stable in comparison to mixtures of N2, H2, and NH3 above approximately 40 GPa. Our results suggest new pathways for synthesis of environmentally benign high energy-density materials. These materials could also exist as alternative planetary ices.",

author = "Goncharov, {Alexander F.} and Nicholas Holtgrewe and Guangrui Qian and Chaohao Hu and Oganov, {Artem R.} and Maddury Somayazulu and Elissaios Stavrou and Pickard, {Chris J.} and Adam Berlie and Fei Yen and Mahmood Mahmood and Lobanov, {Sergey S.} and Zuzana Kon{\^o}pkov{\'a} and Prakapenka, {Vitali B.}",

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year = "2015",

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doi = "10.1063/1.4922051",

language = "英语",

volume = "142",

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T1 - Backbone NxH compounds at high pressures

AU - Goncharov, Alexander F.

AU - Holtgrewe, Nicholas

AU - Qian, Guangrui

AU - Hu, Chaohao

AU - Oganov, Artem R.

AU - Somayazulu, Maddury

AU - Stavrou, Elissaios

AU - Pickard, Chris J.

AU - Berlie, Adam

AU - Yen, Fei

AU - Mahmood, Mahmood

AU - Lobanov, Sergey S.

AU - Konôpková, Zuzana

AU - Prakapenka, Vitali B.

PY - 2015/6/5

Y1 - 2015/6/5

N2 - Optical and synchrotron x-ray diffraction diamond anvil cell experiments have been combined with first-principles theoretical structure predictions to investigate mixtures of N2 and H2 up to 55 GPa. Our experiments show the formation of structurally complex van der Waals compounds [see also D. K. Spaulding et al., Nat. Commun. 5, 5739 (2014)] above 10 GPa. However, we found that these NxH (0.5 < x < 1.5) compounds transform abruptly to new oligomeric materials through barochemistry above 47 GPa and photochemistry at pressures as low as 10 GPa. These oligomeric compounds can be recovered to ambient pressure at T < 130 K, whereas at room temperature, they can be metastable on pressure release down to 3.5 GPa. Extensive theoretical calculations show that such oligomeric materials become thermodynamically more stable in comparison to mixtures of N2, H2, and NH3 above approximately 40 GPa. Our results suggest new pathways for synthesis of environmentally benign high energy-density materials. These materials could also exist as alternative planetary ices.

AB - Optical and synchrotron x-ray diffraction diamond anvil cell experiments have been combined with first-principles theoretical structure predictions to investigate mixtures of N2 and H2 up to 55 GPa. Our experiments show the formation of structurally complex van der Waals compounds [see also D. K. Spaulding et al., Nat. Commun. 5, 5739 (2014)] above 10 GPa. However, we found that these NxH (0.5 < x < 1.5) compounds transform abruptly to new oligomeric materials through barochemistry above 47 GPa and photochemistry at pressures as low as 10 GPa. These oligomeric compounds can be recovered to ambient pressure at T < 130 K, whereas at room temperature, they can be metastable on pressure release down to 3.5 GPa. Extensive theoretical calculations show that such oligomeric materials become thermodynamically more stable in comparison to mixtures of N2, H2, and NH3 above approximately 40 GPa. Our results suggest new pathways for synthesis of environmentally benign high energy-density materials. These materials could also exist as alternative planetary ices.

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DO - 10.1063/1.4922051

M3 - 文章

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SN - 0021-9606

VL - 142

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

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ER -

Backbone N_xH compounds at high pressures

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